Application of fiber reinforced polymer (FRP) cables on long-span cable-supported bridges can overcome the disadvantages of traditional steel cables such as heavy weight, obvious sag effect, decreasing carrying efficiency, pronounced fatigue degradation, and serious corrosion damage. On the basis of theoretical analyses and experimental studies on the application of FRP cable in long-span cable-supported bridges, the research progress in recent years on the key issues of FRP cables in long-span cable-supported bridges is reviewed in detail. The basic mechanical properties of FRP cables, the static and dynamic behavior of long-span cable-supported bridge with FRP cables, and the economic performance of long-span cable-supported bridges with FRP cables are discussed. The results show that FRP cables have the feasibility to be used in long-span cable-supported bridges from the mechanical properties. However, due to the poor shearing and bending performance of FRP cables, abundant nonlinear dynamic behavior, complex dynamic performance of bridges, and insufficient practical experience, the application of FRP cables in long-span cable-supported bridges is facing great difficulties. Accordingly, the future research directions on the application of FRP cables on the long-span cable-supported bridge are addressed.